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Magnetic Switchable Pickering Interfacial Biocatalysis: One-Pot Cascade Synthesis of Phytosterol Esters from High-Acid Value Oil
ACS Sustainable Chemistry & Engineering ( IF 7.1 ) Pub Date : 2021-08-31 , DOI: 10.1021/acssuschemeng.1c02448
Tao Yang 1 , Yufei Zhang 1 , Jing Wang 1 , Fenghong Huang 1 , Mingming Zheng 1
Affiliation  

The traditional reutilization of high-acid value oil resources causes pollution, suffers from high energy consumption, and brings relatively low economic value. In this study, high-acid value oil was converted into high-value product phytosterol esters (PEs) using a “one-pot” enzymatic cascade reaction strategy including the hydrolysis of high-acid value oils into free fatty acids (FFAs) and followed by its esterification of phytosterols. Lipase AYS was immobilized on magnetic hollow mesoporous carbon nanospheres to obtain AYS@MHMCS, forming a sustainable and solvent-free Pickering interfacial biocatalysis platform. Each droplet in the emulsion system served as a microreactor with the reactants in the oil phase; the byproduct glycerol was spontaneously excreted to the aqueous phase which would “push” the hydrolysis reaction forward. The products of hydrolysis (fatty acids) remained in the oil phase, continuing the next esterification reaction with phytosterols, which ensured the efficient and continuous operation of the tandem reaction. Benefiting from the interfacial activation effect of lipase, the catalytic efficiency of the emulsion system was 30 times that of the single-phase system. The yield of PEs was up to 90%, while the highest in the single-phase was only 30%. Additionally, the magnetic-responsive Pickering emulsion could recover AYS@MHMCS intactly in 15 min, and there would be no significant loss of catalytic activity even after continuous reuse for 15 cycles. This method not only provides a robust biocatalysis technique with a sustainable interface but also paves the way to high-value utilization of high-acid value oil resources.

中文翻译:

磁性可切换 Pickering 界面生物催化:从高酸值油中一锅级联合成植物甾醇酯

传统的高酸值石油资源再利用造成污染,能耗高,经济价值相对较低。在这项研究中,使用“一锅”酶促级联反应策略将高酸值油转化为高价值产品植物甾醇酯 (PE),包括将高酸值油水解成游离脂肪酸 (FFA),然后通过植物甾醇的酯化。将脂肪酶 AYS 固定在磁性中空介孔碳纳米球上以获得 AYS@MHMCS,形成可持续且无溶剂的 Pickering 界面生物催化平台。乳液体系中的每一滴都充当与油相中的反应物的微反应器;副产物甘油自发地排泄到水相中,这将“推动”水解反应向前进行。水解产物(脂肪酸)留在油相中,继续与植物甾醇进行下一步的酯化反应,保证了串联反应的高效连续运行。得益于脂肪酶的界面活化作用,乳液体系的催化效率是单相体系的30倍。PEs的产率高达90%,而单相最高只有30%。此外,磁响应 Pickering 乳液可以在 15 分钟内完整地恢复 AYS@MHMCS,即使连续重复使用 15 个循环后催化活性也不会显着损失。该方法不仅提供了一种具有可持续界面的强大生物催化技术,而且为高酸值石油资源的高价值利用铺平了道路。
更新日期:2021-09-13
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